Aerogels are very porous nanostructured materials typically prepared by sol-gel processing. Typical aerogels can exhibit up to 99% porosity, low refractive index (η<1.1) high surface area (>1000 m2/g), and small pores (<10 nm). Aerogels generally comprise dielectric materials such as the oxides of silicon, aluminum and titanium, and can also include organic polymers. Aerogels have many applications including catalyst supports, electrical insulators, thermal insulators, and acoustic insulators. It is desired in many applications to employ an aerogel material as a film (e.g. a layer on the order of 1 um thick) on a substrate (e.g. glass, silicon, metal, ceramic, etc.) in applications ranging from the fabrication of micro-electromechanical (MEM) devices to optical display and solar energy conversion devices. In many of these applications it is required that the aerogel film be patterned on the surface of the substrate, creating sharply defined, exposed areas (e.g. aerogel removed) on the substrate and adjacent unexposed areas (e.g. areas remaining covered by the aerogel layer) on the substrate. Due to the porous nature of the aerogel layer, traditional photolithographic techniques typically produce poorly defined pattern edges between the exposed and unexposed areas of the substrate. What are needed are methods that overcome this limitation and allow the creation of sharply defined patterned features of aerogel layers on the surface of the substrate.